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WO1995009450A1 - Conversion directe de carbone en energie electrique dans une pile a combustible a haute temperature - Google Patents

Conversion directe de carbone en energie electrique dans une pile a combustible a haute temperature Download PDF

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Publication number
WO1995009450A1
WO1995009450A1 PCT/US1994/011088 US9411088W WO9509450A1 WO 1995009450 A1 WO1995009450 A1 WO 1995009450A1 US 9411088 W US9411088 W US 9411088W WO 9509450 A1 WO9509450 A1 WO 9509450A1
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WO
WIPO (PCT)
Prior art keywords
solid electrolyte
fuel
fuel cell
temperature
high temperature
Prior art date
Application number
PCT/US1994/011088
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English (en)
Inventor
Turgut M. Gur
Robert A. Huggins
Original Assignee
The Board Of Trustees Of The Leland Stanford Junior University
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by The Board Of Trustees Of The Leland Stanford Junior University filed Critical The Board Of Trustees Of The Leland Stanford Junior University
Publication of WO1995009450A1 publication Critical patent/WO1995009450A1/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/1233—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte with one of the reactants being liquid, solid or liquid-charged
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • This invention relates to the field of fuel cells, and in particular to the field of high temperature fuel cells for the direct electrochemical conversion of carbon to electrical energy.
  • High temperature fuel cells employing solid electrolytes to convert the chemical energy stored in gaseous fuels to electrical energy have been reported.
  • oxygen is the working medium for electrochemical conversion, moving as oxide ions across the solid electrolyte to react with gaseous fuels such as coal derived gases, H2 , and CH4.
  • Gaseous fuels such as coal derived gases, H2 , and CH4.
  • Electrons consumed in the reduction of oxygen to oxide ions at the cathode side of the electrolyte are released from the oxide ions at the anode side of the electrolyte to generate current flow in an external circuit.
  • These fuel cells operate most efficiently when the gaseous fuels are completely oxidized at the anode to CO2 and H2O in the case of carbon containing fuels or H2O in the case of H2.
  • the efficiency of solid oxide fuel cells is also improved by operating them at high temperatures where ohmic losses due to the impedances of the solid electrolyte and the electrode are minimized.
  • coal as a carbon source in solid oxide fuel cells.
  • a separate gasification step is employed to convert the coal into a gaseous fuel prior to the combustion process.
  • this is done by passing wet oxygen ( O2 plus H2O) over coal at elevated temperatures to generate CO and H2, and the CO is subsequently reacted with O2 to produce CO2.
  • O2 plus H2O wet oxygen
  • the combustion of coal using this intermediate conversion process is still less efficient than the direct combustion of coal.
  • the gasification process used to generate CO for electrochemical conversion is a thermal process, and therefore subject to the energy conversion limits of the Carnot cycle.
  • the primary reaction at the anode of the fuel cell is the oxidation of CO to CO2, which yields approximately half as much chemical energy for conversion to electricity as the oxidation of C to CO2.
  • the present invention is a high temperature fuel cell (10) that uses an oxide ion conducting solid electrolyte (30) in conjunction with separate temperate zones (14, 16) to optimize the direct electrochemical conversion of carbon fuels (12) to electrical energy.
  • the high temperature fuel cell (10) of the present invention eliminates the need for an intermediate step in which the carbon fuel (12) is converted into a gaseous fuel prior to combustion. Combustion efficiency is optimized by providing fuel cell (10) with separate temperature zones (14, 16) for the carbon fuel (12) and the solid electrolyte (30), respectively, allowing simultaneous and independent control of the reactions which drive the electrochemical process and the ionic conductivity of the solid electrolyte (30).
  • a high temperature fuel cell (10) comprises a first heat source (22), a second heat source (26), and housing (18), which includes a non-porous section (15) and a solid electrolyte (30).
  • the solid electrolyte (30) has first and second electrolyte surfaces (32, 34) on which are deposited first (anode) and second (cathode) electrodes (36, 38), respectively, for conducting currents generated by high temperature fuel cell (10).
  • the first heat source (22) is located in the vicinity of solid electrolyte (30) of housing (18) to establish a first temperature zone (14) of fuel cell (10).
  • the second heat source (26) is positioned in the vicinity of the non-porous section (15) of housing (18) at a location that is removed from first heat source (22), to establish a second temperature zone (16) in fuel cell (10).
  • a fuel compartment (20) which communicates between the first and second temperatures zones (14, 16) is formed in housing (18) by the non-porous section (15) and the first electrolyte surface (32) of solid electrolyte (30).
  • the fuel compartment (20) includes a gas inlet (25) and may include a liquid seal (24) for adjusting the pressure in the fuel compartment (20).
  • Electrical power is generated from the high temperature fuel cell (10) by placing carbon fuel (12) in the second temperature zone (16) of the fuel compartment (20) and heating the carbon fuel (12) to a temperature that favors complete oxidation of the carbon fuel (12) to CO2 .
  • First temperature zone (14) is adjusted by means of first heat source (22) to a temperature at which ohmic losses due to the impedances of the solid electrolyte (30) and electrodes (36, 38) are minimized.
  • Oxygen is then provided to the carbon fuel (12) by supplying an oxygen containing gas to the second electrode (38) of the solid electrolyte (30), the driving force for conduction of oxide ions through the solid electrolyte (30) being provided by the difference between the activities of oxygen in the fuel compartment (20) and in the oxygen containing gas supplied to the second electrode (38).
  • a high temperature fuel cell (60) may be implemented for commercial purposes using a fluidized bed reactor (50) for the fuel compartment (20). In a fluidized bed reactor (50), fine particles of carbon fuel (12) are suspended by blowing a non-reactive gas in through the bottom (52) of the reactor (50). Second heat sources (26) are located along the outer surface of the reactor (50) to maintain the carbon fuel (12) at the desired temperature.
  • Fig. 1A is a diagram of a cross-section of one embodiment of a high temperature fuel cell (10) in accordance with the present invention.
  • Fig. IB is a diagram of a cross section of another embodiment of a high temperature fuel cell (10) in accordance with the present invention.
  • Fig. 2 is a diagram of the theoretical activities of oxygen as a function of temperature for the partial and complete oxidation of a carbon fuel (12).
  • Fig. 3 is a diagram of d e expected and measured (squares) open circuit voltages generated between the electrodes (36, 38) of the high temperature fuel cell (10) of Fig. 1A as a function of the temperature of the carbon fuel (12).
  • Fig. 4 is a diagram of a high temperature fuel cell (60) in accordance with the present invention where the non-porous section (15) of housing (18) is a fluidized bed reactor (50).
  • Fig. 5 is a diagram of a high temperature fuel cell (70) in accordance with the present invention comprising a collection of high temperature fuel cells (10) positioned in a container vessel (74).
  • a high temperature fuel cell 10 for efficiently converting the chemical energy of carbon directly into electrical energy by electrochemical means fuel cell 10 comprises a first heat source 22, a second heat source 26, and a housing 18 which includes a non-porous section 15 and a solid electrolyte 30.
  • Solid electrolyte 30 has a first electrolyte surface 32 which is in electrical contact with a first electrode 36, and a second electrolyte surface 34 which is in electrical contact with a second electrode 38.
  • Electrical connections 35, 37 are in electrical contact with first and second electrodes 36, 38, respectively, for conducting electrical current generated by fuel cell 10.
  • First heat source 22 is positioned in the vicinity solid electrolyte 30 to establish a first temperature zone 14 in the vicinity of solid electrolyte 30.
  • Second heat source 24 is located in the vicinity of non-porous section 15 at some distance removed from first heat source 22 to establish a second temperature zone 16.
  • First and second heaters 22, 26 may be for example resistive heating elements or radiative heaters arrayed circumferentially around housing 18.
  • First and second temperature zone 14, 16 are not sharply defined, but rather gradually merge one into the other.
  • Non-porous section 15 of housing 18 and first electrolyte surface 32 of solid electrolyte 30 together define a fuel compartment 20, which spans first and second temperature zones 14, 16 so that oxygen from solid electrolyte 30 and carbon fuel 12 may pass freely between first and second temperature zones 14, 16.
  • the geometry of fuel cell 10 and the relative sizes of first and second temperature zones 14, 16 are selected so that the temperature of carbon fuel 12 is determined primarily by the temperature of second temperature zone 16.
  • a gas inlet 25 and a liquid seal 24 may be provided for purging fuel compartment 20 and maintaining the pressure in fuel compartment 20 at a constant level during combustion.
  • solid electrolyte 30 has a cylindrical shape and extends into non-porous section 15 so that first electrode 36 at closed end 40 is within first temperature zone 14 and proximate to second temperature zone 16.
  • An oxygen containing gas such as air or pure oxygen is supplied to second electrode 38 of solid electrolyte 30, where it is oxidized and transported across solid electrolyte 30 to first electrode 26 as oxide ions.
  • oxygen is regenerated by reduction of the oxide ions, and made available for combustion by carbon fuel 12 in fuel compartment 20.
  • the geometry of solid electrolyte 30 in Fig 1 A enhances the intermixing of oxygen provided through solid electrolyte 30 with carbon fuel 12.
  • Fig. IB there is shown an alternative embodiment of high temperature fuel cell 10, wherein solid electrolyte 30 and housing 18 together form an elongated fuel cell 10.
  • Oxygen is provided to carbon fuel 12 by supplying an oxygen containing gas to solid electrolyte 30, where its oxidation and reduction at second and first electrodes 38, 36, respectively, generates electrical current which is collected by connections 35, 37.
  • a Non-reactive gas such as for example CO2, N2, Ar, or He entering fuel cell 10 at first end 17 of housing 18 may be used to entrain carbon fuel 12 in second temperature zone 16 and transport it toward solid electrolyte 30 for reaction with oxygen. Non-reactive gas and any unreacted carbon fuel 12 or oxygen will exit temperature fuel cell 10 at second end 19 of housing 18.
  • a return line 31 may be provided to allow for recirculation of reactants through temperature fuel cell 10.
  • Non-porous section 15 provides structural support for solid electrode 30 and together with solid electrolyte 30 forms fuel compartment 20.
  • Non-porous section 15 may be selected from among refractory materials that are oxidation and reduction resistant and that do not display the mixed electronic and ionic conducting properties discussed below.
  • non-porous section 15 may be a ceramic material or an oxidation resistant metal or alloy.
  • solid electrolytes 30 for use in fuel cells 10 in accordance with the present invention are ionic conductors and electronic insulators, since the greater conductivity of electrons would otherwise effectively eliminate any charge conduction by oxide ions.
  • Suitable solid electrolytes 30 may be generated for example by doping the oxides of Bi, Zr, Hf, Th, and Ce with either alkaline earth oxides such as CaO or MgO, or rare-earth oxides such as SC2O3, Y2O3, or Yb2 ⁇ 3. Solid electrolytes are discussed below in conjunction with the temperature dependence of their conductivities.
  • Second electrode 38 the cathode of fuel cell 10, provides a pathway for the electrons necessary to reduce oxygen to oxide ions for transport across solid electrolyte 30.
  • First electrode 36 the anode of fuel cell 10, provides a pathway to conduct away electrons released by the oxidation of oxide ions.
  • Oxygen is provided to second electrolyte surface 34 of solid electrolyte 30 by directing either an oxygen-containing gas or pure oxygen at electrode 38, where the oxygen is reduced to oxide ions.
  • Electrode 38 must thus allow the mass transport of oxygen in the form of oxide ions between the oxygen-containing gas and second electrolyte surface 34 of solid electrolyte 30.
  • electrode 36 must allow oxide ions to pass from first electrolyte surface 32 of solid electrolyte 30 into electrode 36 to be oxidized.
  • electrodes 36, 38 are typically made by applying a porous metallic paste to first and second electrolyte surfaces 32, 4 of solid electrolyte 30.
  • the porous metallic paste is made from an oxidation resistant metal such as a noble metal.
  • a porous platinum paste is used to make electrode 38, the reduction of molecular oxygen to oxide ions occurs at three phase line boundaries where solid electrolyte 30, electrode 38, and the oxygen-containing gas all come into direct contact.
  • electrode 38 is made from a mixed conducting oxide material, since such materials are capable of conducting both oxide ions and electronic species (electrons or holes).
  • first and second electrolyte surfaces 32, 34 can be completely coated with mixed conducting oxide electrodes 36, 38, respectively.
  • the mixed conducting properties of the oxide allows electrodes 36, 8 to conduct not only the electrons necessary for the reduction/oxidation reactions but also to conduct the oxide ions to and from the underlying solid electrolyte 30.
  • Suitable mixed conducting oxide materials may be selected from a variety of oxides, including those having perovskite, pyrochlore, sheelite, and rutile structures.
  • mixed conducting perovskites may be selected from compositions having the formulas:
  • La ⁇ x Sr x C ⁇ yFe ⁇ _y ⁇ 3 (Eq. II), where x is between zero and one, and y is also between zero and one.
  • two principal means of energy loss must be effectively controlled. These are the incomplete oxidation of carbon fuel 12 and the ohmic losses created by transporting oxide ions across solid electrolyte 30 and electrodes 36, 8 having finite impedances. In the first case, less oxygen is consumed and less energy is generated for conversion to electricity when carbon fuel 12 is incompletely oxidized. In the second case, additional energy generated by electrochemical conversion of carbon fuels 12 is consumed in moving charges through solid electrolyte 30. Temperature zones 14, 16 created by heat sources 22, 26 provide means to optimize operation of fuel cell 10 in view of these inefficiencies. In the simplest case of a pure carbon fuel 12, combustion occurs by two different reactions. These reactions are the partial oxidation of carbon to CO:
  • carbon fuel 12 contains hydrogen and for example sulfur impurities, water and oxides of sulfur are also produced during oxidation. More generally, carbon fuels 12 such as coal may contain volatile impurities such as hydrogen and hydrocarbon compounds in addition to sulfur and ash. While many of these impurities can be removed by coking or desulfurization pretreatments, fuel cells 10 in accordance with the present invention may use untreated coal as carbon fuel 12, the combustible impurities being oxidized along with carbon fuel 12.
  • the reaction of Eq IN is preferred since it consumes more oxygen and makes available more chemical energy for conversion to electrical current. However, both reactions will occur during combustion of carbon fuel 12, and the degree to which the reaction of Eq. IV predominates over the reaction of Eq. Ill depends in part on the temperature at which the reactions occur.
  • Fig. 2 there is shown a graph of the theoretical activity of O2 as a function of the reaction temperature for the reactions of Eq. El and IN.
  • the reaction of Eq. IN is favored at temperatures below about 1000° K (approximately 700° C) and that the predominance of the reaction of Eq. IV over the reaction of Eq. HI increases as the temperature of the reactants is decreased.
  • combustion of carbon fuel 12 to completion will be more favored thermodynamically the more the reactant temperatures are reduced below about 700° C.
  • the temperature of fuel compartment 20 must still be kept high enough so that the reaction of Equation IV proceeds at a reasonable rate.
  • the reactants are maintained at about 700° C by using heat source 22 to adjust the temperature of fuel compartment 20.
  • Another factor affecting the rates of reaction of Eqs. IE and IV is the amount of carbon available to react with the O2. Where carbon is the limiting reactant in the combustion of carbon fuel 12 as may be the case where a solid carbon fuel 12 is used, O2 will be in excess. Consequently, the activity of the O2 increases, decreasing the chemical driving force that generates electric current. This effect can be countered by making a solid carbon fuel 12 available to O2 in a more reactive form.
  • carbon fuel 12 is in the form of a solid carbon such as coal or graphite, it is preferably provided in the form of a finely divided powder.
  • the second factor that may reduce the efficiency of fuel cell 10 is the ohmic loss attributable to the conduction of oxide ions through solid electrolyte 30 and electrodes 36, 38.
  • Solid electrolytes 30 having sufficient ionic conductivities for use in fuel cells 10 may be obtained for example by doping oxides of Bi, Zr, Hf, Th, and Ce with either alkaline earth oxides such as CaO or MgO, or a rare-earth oxide such as SC2O3, Y2O3, or Yb2 ⁇ 3.
  • alkaline earth oxides such as CaO or MgO
  • a rare-earth oxide such as SC2O3, Y2O3, or Yb2 ⁇ 3.
  • the actual ionic conductivities of solid electrolyte 30 will depend on the temperature at which solid electrolyte 30 is maintained.
  • the ionic conductivity of Zr ⁇ 2 stabilized by SC2O3 increases from approximately 0.01 ⁇ ⁇ * cm ⁇ l at 650° C to approximately 0.1 ⁇ ⁇ l cm ⁇ l at 900° C.
  • fuel cells 10 operated at about 650° C will have ohmic losses due to I- ⁇ R heating that are approximately an order of magnitude greater than fuel cells 10 operated at 900° C, making it more efficient to operate at higher temperatures.
  • solid electrolyte 30 is Y2O3 stabilized Zr ⁇ 2
  • fuel cell 10 is typically operated at temperatures above about 800° C. This is accomplished in fuel cells 10 of the present invention by using first heat source 22 to adjust first temperature zone 14 around solid electrolyte 30.
  • first heat source 22 to adjust first temperature zone 14 around solid electrolyte 30.
  • a fuel cell 60 comprising a fluidized bed reactor 50 having a collection of solid electrolytes 30 mounted in a wall 56.
  • Each of solid electrolytes 30 has first and second electrolyte surfaces 32, 34 which are in electrical contact with first and second electrodes 36, 38, respectively. Electrodes 36, 38 from each solid electrolyte 30 may be connected in series or in parallel, according to the use to which fuel cell 60 is applied.
  • Fluidized bed reactor 50 includes a bottom surface 52 having gas inlets 25.
  • fine particles of carbon fuel 12 are introduced into fuel compartment 20 of fluidized bed reactor 50.
  • a stream of non-reactive gas is blown in through gas inlets 25 to distribute fine particles of carbon fuel 12 throughout fuel compartment 20.
  • a gas outlet 27 allows the pressure of non-reactive gas in fuel compartment 20 to be controlled.
  • fuel cell 60 includes first heat source 22 for adjusting temperature zone 14 in the vicinity of solid electrolytes 30 and second heat source 26 for adjusting the temperatures of carbon fuel 12.
  • a fuel cell 70 comprising a collection of fuel cells 10 as shown in Fig IB.
  • fuel cell 70 has a gas line 72 for recirculating a non-reactive gas through fuel cells 10, to maximize mixing of carbon fuel 12 and oxygen form solid electrolytes 30 and minimize loss of uncombusted carbon fuel 12.
  • a gas inlet 76 allows an oxygen containing gas to be introduced into a container vessel 74, where it is provided to solid electrolytes 30.
  • First and second heat sources 22, 26 establish first and second temperature zone 14, 16 for solid electrolytes 30 and carbon fuel 12.
  • Electrical leads 35, 37 from first and second electrolyte surfaces 36, 38, respectively, of solid electrolytes 30 are connected to sum the current generated by individual fuel cells 10 and provide more power.

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Abstract

Pile à combustible à haute température (10) présentant une première et une seconde zone de température (14, 16), assurant la conversion directe d'un combustible carboné (12) et comportant une première et une seconde source de chaleur (22, 26) et une enceinte (18) comprenant une zone non poreuse (15) et un électrolyte solide (30) présentant une première et une seconde surface de contact avec l'électrolyte (32, 34) auxquelles la première et la seconde électrode (36, 38) sont raccordées électriquement. La première source de chaleur (26) crée une première zone de température (14) au voisinage de l'électrolyte solide (30) permettant de régler la conductivité dudit électrolyte (30) et des électrodes (36, 38). La seconde source de chaleur (26) est placée au voisinage de la zone non poreuse (15) de l'enceinte (18) et distante de la première source de chaleur (22) et crée une seconde zone de température. Un compartiment à combustible (20) délimité par la première surface (32) de l'électrolyte solide (30) et par la partie non poreuse (15) de l'enceinte (18) englobe la première et la seconde zones de température (14, 16) pour permettre le mélangeage de l'oxygène fourni par l'électrolyte solide (30) et le combustible carboné localisé au départ dans la seconde zone de température (16). Le compartiment à combustible (20) peut comporter un orifice d'entrée du gaz (25), un orifice de sortie du gaz et une canalisation de retour (31) servant à la recirculation du gaz n'ayant pas réagi de façon à renforcer le mélangeage de l'oxygène et du combustible carboné (12). Pour la production de courant, on règle la température de la seconde zone de température à un niveau qui favorise la complète oxydation du combustible (12), et celle de la première zone de température (14) à un niveau qui réduit la résistance de l'électrolyte solide (30) et des électrodes (36, 38) et on fournit de l'oxygène à la seconde surface (32) de l'électrolyte solide (30) par apport d'un gaz riche en oxygène.
PCT/US1994/011088 1993-09-30 1994-09-29 Conversion directe de carbone en energie electrique dans une pile a combustible a haute temperature WO1995009450A1 (fr)

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US08/129,948 1993-09-30
US08/129,948 US5376469A (en) 1993-09-30 1993-09-30 Direct electrochemical conversion of carbon to electrical energy in a high temperature fuel cell

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EP1702380A4 (fr) * 2003-11-14 2008-12-31 Univ Akron Pile a combustible a base de carbone
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US8877136B1 (en) 2012-09-05 2014-11-04 Andrei Razumau Method of producing synthesis gas from coal
US9780424B2 (en) 2012-09-21 2017-10-03 Danmarks Tekniske Universitet Rechargeable carbon-oxygen battery
CN103441294B (zh) * 2013-09-13 2015-08-19 哈尔滨工业大学 采用含碳垃圾作为sofc燃料的发电装置

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US7678484B2 (en) 2000-04-18 2010-03-16 Celltech Power Llc Electrochemical device and methods for energy conversion
US7943271B2 (en) 2000-04-18 2011-05-17 Celltech Power Llc Electrochemical device and methods for energy conversion
US7229710B2 (en) 2001-11-20 2007-06-12 Celltech Power, Inc. Electrochemical system and methods for control thereof
US7745064B2 (en) 2003-06-10 2010-06-29 Celltech Power Llc Oxidation facilitator
US7943270B2 (en) 2003-06-10 2011-05-17 Celltech Power Llc Electrochemical device configurations

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